基于镧系金属有机框架材料检测水体中酰胺类除草剂残留的可视化技术研究
投稿时间：2019-04-12      点此下载全文 HTML
引用本文：汪海英,刘剀,高立娣,等.基于镧系金属有机框架材料检测水体中酰胺类除草剂残留的可视化技术研究[J].农药学学报,2019,21(4):461-467.
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作者单位E-mail
汪海英 浙江大学 环境与资源学院, 浙江 杭州 310000  
刘剀 加州理工学院 环境科学与工程系, 美国帕萨迪纳 加州 91126  
高立娣 齐齐哈尔大学 化学与化学工程学院, 黑龙江 齐齐哈尔 161006 gaolidi@163.com 
刘维屏 浙江大学 环境与资源学院, 浙江 杭州 310000 wliu@zju.edu.cn 
基金项目:国家自然科学基金（21777137）
中文摘要:研发水体中酰胺类农药残留简便快捷的检测技术，对评估农药造成的水体污染和提出相应的治理对策具有重要意义。以共掺杂镧系金属离子（Eu3+ 和Tb3+）作为配位金属离子，分别利用水热法和微波法制备了镧系金属有机框架材料（lanthanide metal-organic frameworks，Ln-MOF），对其结构和性质进行了表征，并采用所制备的Ln-MOF对水体中残留的5种常见酰胺类除草剂（乙草胺、异丙草胺、丙草胺、敌草胺和异丙甲草胺）进行了定性和定量分析。结果表明：与水热法相比，采用微波法制备的Ln-MOF样品呈蓬松的簇状、结晶度好，且具有更高的发光效率，故选择微波法制备Ln-MOF。农药残留检测试验结果表明，不同除草剂对Tb3+和Eu3+的发光会产生差别性猝灭，并使整体发射光发生变化，进而实现水体中农药的可视化检测。进一步研究发现，荧光强度比值I（Tb3+）/I（Eu3+）与丙草胺浓度在0.1~1 mmoL/L范围时呈线性相关，线性相关系数R2 = 0.998，检测限（LOD）为0.08 mmoL/L。另外，该材料对于用湖水配制的除草剂溶液也具有一定的定性检测能力。本研究结果展现了Ln-MOF用于水体中酰胺类除草剂的定性、定量分析具有良好应用前景。
中文关键词:镧系金属离子  金属有机框架材料  酰胺类除草剂  荧光传感  可视化检测  定性和定量分析
 
Research on visual detection of the residues of amide herbicides in water using lanthanide metal-organic framework
Abstract:Convenient detection of amide herbicides in water is essential for assessing the herbicide pollution and proposing the corresponding countermeasures. In this work, Eu3+ and Tb3+ co-doped lanthanide metal-organic frameworks (Ln-MOF) were prepared using hydrothermal and microwave methods respectively. Their structure and optical properties were also characterized. Then the synthesized material was applied to the analysis of five amide herbicides (acetochlor, propisochlor, pretilachlor, napropamide and metolachlor) in water qualitatively and quantitatively. Results showed that the Ln-MOF prepared by microwave synthesis method was fluffy clusters with good crystallinity and high luminous efficiency. Therefore, the microwave synthesis method was selected. Test results show that diverse herbicides quench the fluorescence of Tb3+ and Eu3+ differently, which can change the color of emission light, then realizing the visual detection of amide herbicides in water. Further, when the concentration of pretilachlor is between 0.1 to 1 mmoL/L, the emission intensity ratio of I (Tb3+)/I (Eu3+) increased with increase of the concentration of pretilachlor, with a correlation coefficient of R2=0.998. The limit of detection is 0.08 mmoL/L. Moreover, Ln-MOF can also be used for the qualitative analysis of the herbicide in lake water. These results indicated potential application of Ln-MOF for the qualitative and quantitative analysis of amide herbicides in water.
Key words:lanthanide ions  metal organic-framework material  amide herbicides  fluorescence sensing  visual detection  qualitative and quantitative analysis
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